模拟核素固化体Gd2Zr2-xCexO7(0≤ x≤ 2.0)的物相及化学稳定性研究

卢喜瑞; 董发勤; 胡淞; 王晓丽; 吴彦霖

doi:10.7498/aps.61.152401

摘要

为研究钆锆烧绿石固化Pu(Ⅳ)的相变化情况及化学稳定性, 以Gd2O3, ZrO2为原料, Ce(Ⅳ)作为Pu(Ⅳ)的模拟替代物质, 采用冷压热烧结的方法制备出Gd2Zr2-xCexO7(0≤ x≤ 2.0)系列样品. 分别在40 °C和70 °C的合成海水中, 对固化体的长期浸出性能进行研究. 借助粉末X射线衍射仪对所制备样品的物相信息进行收集, 利用等离子体质谱仪对固化体的浸出浓度数据进行分析. 研究结果表明: 当x ≤0.08时, 固化体保持为烧绿石相; 当x>0.08时, 固化体转变为具有缺陷的萤石型结构相. 固化体中Gd3+, Zr4+和Ce4+在合成海水中, 随着浸泡时间的延长浸出浓度逐渐上升, 70 °C下的浸出浓度高于40 °C下的浸出浓度. 在42 d时, 固化体中Gd3+的最大浸出浓度在0.032 μg·ml-1以下, Zr4+的最大浸出浓度在0.003 μg·ml-1以下; Ce4+的最大浸出浓度在0.032 μg·ml-1以下.

关键词:

烧绿石 /
固化体 /
物相 /
化学稳定性

Abstract

In order to investigate phase change and chemical stability of pyrochlore Gd2Zr2O7 used for immobilizing Pu(Ⅳ), tetravalent cerium is used as the simulacrums for plutonium with tetravalence, and Gd2Zr2-xCexO7(0≤ x≤ 2.0) series samples are successfully synthesized by high temperature solid reaction and using Gd2O3 and ZrO2 powders as starting materials. The experiments of long-term chemical stability are conducted in synthetic seawater at 40 °C and 70 °C separately. The XRD diffractive data and extraction ratio of as-gained samples are collected by the help of X-ray diffraction (XRD) instrument and inductively coupled plasma mass spectrometry. The results indicate that the phases of compounds change from pyrochlore to fluorite-type phase when the value of x is more than 0.08. Extraction ratios of Gd3+, Zr4+ and Ce4+ in waste forms increase with the increase of immersion time in synthetic seawater. The extraction ratio of waste form at 70 °C is higher than at 40 °C. The highest extraction ratios of Gd3+, Zr4+ and Ce4+ for 42 days are no more than 0.032, 0.003 and 0.032 μg·ml-1 respectively.

Keywords:

作者及机构信息

1.
四川大学原子核科学技术研究所, 成都 610064;

2.
西南科技大学核废物与环境安全国防重点学科实验室, 绵阳 621010;

3.
中国工程物理研究院核物理与化学研究所, 绵阳 621900;

4.
日本国立综合研究大学院大学, 三浦郡 240-0193

基金项目: 国家高技术研究发展计划(863)计划重点项目(批准号: 2009AA050703), 国家自然科学基金青年科学基金(批准号: 21007052), 四川大学辐射物理及技术教育部重点实验室基金(批准号: 2011-03), 西南科技大学核废物与环境安全国防重点学科实验室基金(批准号: 11zxnk09)和西南科技大学青年基金(批准号: 11zx3108)资助的课题.

Authors and contacts

1.
Institute of Nuclear Science and Technology, SU, Chengdu 610064, China;

2.
National Defense Key Discipline Lab of Nuclear Waste and Environmental Safety, SWUST, Mianyang 621010, China;

3.
Institute of Nuclear Physics and Chemistry, CAEP, Mianyang 621900, China;

4.
Graduate University for Advanced Studies, Hayama 240-0193, Japan

Funds: Project supported by the Key Project of National High Technology Research and Development Program (863Program) of China (Grant No. 2009AA050703), the Young Scientists Fund of National Natural Science Foundation of China (Grant No. 21007052), the Foundation of Key Laboratory of Radiation Physics and Technology (Sichuan University), Ministry of Education of China (Grant No. 2011-03), the Foundation of Key Subject Laboratory of National Defense for Radioactive Waste and Environmental Security (Southwest University of Science and Technology) (Grant No. 11zxnk09), and the Youth Foundation of Southwest University of Science and Technology (Grant No. 11zx3108).

参考文献

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施引文献

[1]	Hatch L P 1953 American Scientist 41 410
[2]	Ringwood A E, Kesson S E, Ware N G, Hibberson W, Major A 1979 Nature 15 278
[3]	Clarke D R 1983 Annual Review of Materials Science 13 191
[4]	Robert L E J 1990 Annual Review of Nuclear and Particle Science 40 79
[5]	Donald I W, Metcalfe B L, Taylor R N J 1997 Journal of Materials Science 32 5851
[6]	Weber W J, Ewing R C, Angell C A, Arnold G W, Cormack A N, Delaye J M, Griscom D L, Hobbs L W, Navrotsky. A, Price D L, Stoneham A M, Weinberg M C 1997a Journal of Materials Research 12 1946
[7]	Weber W J, Ewing R C, Angell C A 1998 Journal of Materials Research 13 1434
[8]	Wang S X, Begg B D, Wang L M, Ewing R C, Weber W J, Govidan Kutty K V 1999 Journal of Materials Research 14 4470
[9]	Weber W J, Ewing R C 2000 Science 289 5487
[10]	Ewing R C, Weber W J, Lian J 2004 Journal of Applied Physics 95 5949
[11]	Lu X R, Cui C L, Zhang D, Chen M J, Yang Y K 2011 Acta Phys. Sin. 60 078901 (in chinese) [卢喜瑞, 崔春龙, 张东, 陈梦君, 杨岩凯 2011 60 078901]

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